scholarly journals The size-composition distribution of atmospheric nanoparticles over Europe

2018 ◽  
Author(s):  
David Patoulias ◽  
Christos Fountoukis ◽  
Ilona Riipinen ◽  
Ari Asmi ◽  
Markku Kulmala ◽  
...  
Keyword(s):  
Ultrafine Particles ◽  
Transport Model ◽  
Ultrafine Particle ◽  
Three Dimensional ◽  
Size Composition ◽  
Ground Level ◽  
Basis Set ◽  
Chemical Transport Model ◽  
Airborne Measurements ◽  
Po Valley

Abstract. PMCAMx-UF, a three-dimensional chemical transport model focusing on the simulation of the ultrafine particle size distribution and composition has been extended with the addition of the volatility basis set (VBS) approach for the simulation of organic aerosol (OA). The model was applied in Europe to quantify the effect of secondary semi-volatile organic vapors on particle number concentrations. The model predictions were evaluated against field observations collected during the PEGASOS-2012 campaign. The measurements included both ground and airborne measurements, from stations across Europe and a Zeppelin measuring above Po-Valley. The ground level concentrations of particles larger than 100 nm (N100) were reproduced with a daily normalized mean error of 40 % and a daily normalized mean bias of −20 %. PMCAMx-UF tended to overestimate the concentration of particles larger than 10 nm (N10) with a daily normalized mean bias of 75 %. The model performed quite well compared to the Zeppelin measurements, reproducing more than 85 % of N10 and 75 % of the N100 data, within a factor of 2. The condensation of organics led to an increase (50–120 %) of the N100 concentration mainly in central and northern Europe, while the N10 concentration decreased by 10–30 %. Including the VBS in the PMCAMx-UF improved its ability to simulate aerosol number concentration compared to simulations neglecting organic condensation on ultrafine particles.

scholarly journals Simulation of the size-composition distribution of atmospheric nanoparticles over Europe

2018 ◽  
Vol 18 (18) ◽  
pp. 13639-13654 ◽  
Author(s):  
David Patoulias ◽  
Christos Fountoukis ◽  
Ilona Riipinen ◽  
Ari Asmi ◽  
Markku Kulmala ◽  
...  
Keyword(s):  
Ultrafine Particles ◽  
Transport Model ◽  
Ultrafine Particle ◽  
Three Dimensional ◽  
Size Composition ◽  
Ground Level ◽  
Basis Set ◽  
Chemical Transport Model ◽  
Airborne Measurements ◽  
Po Valley

Abstract. PMCAMx-UF, a three-dimensional chemical transport model focusing on the simulation of the ultrafine particle size distribution and composition has been extended with the addition of the volatility basis set (VBS) approach for the simulation of organic aerosol (OA). The model was applied in Europe to quantify the effect of secondary semi-volatile organic vapors on particle number concentrations. The model predictions were evaluated against field observations collected during the PEGASOS 2012 campaign. The measurements included both ground and airborne measurements, from stations across Europe and a zeppelin measuring above Po Valley. The ground level concentrations of particles with a diameter larger than 100 nm (N100) were reproduced with a daily normalized mean error of 40 % and a daily normalized mean bias of −20 %. PMCAMx-UF tended to overestimate the concentration of particles with a diameter larger than 10 nm (N10) with a daily normalized mean bias of 75 %. The model was able to reproduce, within a factor of 2, 85 % of the N10 and 75 % of the N100 zeppelin measurements above ground. The condensation of organics led to an increase (50 %–120 %) in the N100 concentration mainly in central and northern Europe, while the N10 concentration decreased by 10 %–30 %. Including the VBS in PMCAMx-UF improved its ability to simulate aerosol number concentration compared to simulations neglecting organic condensation on ultrafine particles.

scholarly journals Simulation of the effects of low volatility organic compounds on aerosol number concentrations in Europe

2021 ◽  
Author(s):  
David Patoulias ◽  
Spyros N. Pandis
Keyword(s):  
Organic Compounds ◽  
Transport Model ◽  
Ultrafine Particle ◽  
Three Dimensional ◽  
Ground Level ◽  
Chemical Transport Model ◽  
Organic Vapors ◽  
Chemical Aging ◽  
Po Valley ◽  
Small Change

Abstract. PMCAMx-UF, a three-dimensional chemical transport model focusing on the simulation of the ultrafine particle size distribution and composition has been extended with the addition of reactions of chemical aging of semi-volatile anthropogenic organic vapors, the emissions and chemical aging by intermediate volatile organic compounds (IVOCs) and the production of extremely low volatility organic compounds (ELVOCs) by monoterpenes. The model is applied in Europe to quantify the effect of these processes on particle number concentrations. The model predictions are evaluated against both ground measurements collected during the PEGASOS 2012 summer campaign across many stations in Europe and airborne observations by a Zeppelin measuring above Po-Valley, Italy. PMCAMx-UF reproduces the ground level daily average concentrations of particles larger than 100 nm (N100) with normalized mean error (NME) of 45 % and normalized mean bias (NMB) close to 10 %. For the same simulation, PMCAMx-UF tends to overestimate the concentration of particles larger than 10 nm (N10) with a daily NMB of 23 % and a daily NME of 63 %. The model was able to reproduce more than 75 % of the N10 and N100 airborne observations (Zeppelin) within a factor of 2. The ELVOC production by monoterpenes is predicted to lead to surprisingly small changes of the average number concentrations over Europe. The total number concentration decreased due to the ELVOC formation by 0.2 %, the N10 decreases by 1.1 %, while N50 increased by 3 % and N100 by 4 % due to this new SOA source. This small change is due to the nonlinearity of the system with increases predicted in some areas and decreases in others, but also the cancelation of the effects of the various processes like accelerated growth and accelerated coagulation. Locally, the effects can be significant. For example, an increase in N100 by 20–50 % is predicted over Scandinavia and significant increases (10–20 %) over some parts of central Europe. The ELVOCs contributed on average around 0.5 μg m−3 and accounted for 10–15 % of the PM2.5 OA. The addition of IVOC emissions and their aging reactions led to surprising reduction of the total number of particles (Ntot) and N10 by 10–15 and 5–10 %, respectively, and to an increase of the concentration of N100 by 5–10 %. These were due to the accelerated coagulation and reduced nucleation rates.

scholarly journals Evaluation of a three-dimensional chemical transport model (PMCAMx) in the European domain during the EUCAARI May 2008 campaign

2011 ◽  
Vol 11 (20) ◽  
pp. 10331-10347 ◽  
Author(s):  
C. Fountoukis ◽  
P. N. Racherla ◽  
H. A. C. Denier van der Gon ◽  
P. Polymeneas ◽  
P. E. Charalampidis ◽  
...  
Keyword(s):  
Time Resolution ◽  
Transport Model ◽  
Three Dimensional ◽  
Model Performance ◽  
Ground Level ◽  
Chemical Transport ◽  
Organic Aerosol ◽  
High Time Resolution ◽  
Chemical Transport Model ◽  
Airborne Measurements

Abstract. PMCAMx-2008, a detailed three-dimensional chemical transport model (CTM), was applied to Europe to simulate the mass concentration and chemical composition of particulate matter (PM) during May 2008. The model includes a state-of-the-art organic aerosol module which is based on the volatility basis set framework treating both primary and secondary organic components as semivolatile and photochemically reactive. The model performance is evaluated against high time resolution aerosol mass spectrometer (AMS) ground and airborne measurements. Overall, organic aerosol is predicted to account for 32% of total PM1 at ground level during May 2008, followed by sulfate (30%), crustal material and sea-salt (14%), ammonium (13%), nitrate (7%), and elemental carbon (4%). The model predicts that fresh primary OA (POA) is a small contributor to organic PM concentrations in Europe during late spring, and that oxygenated species (oxidized primary and biogenic secondary) dominate the ambient OA. The Mediterranean region is the only area in Europe where sulfate concentrations are predicted to be much higher than the OA, while organic matter is predicted to be the dominant PM1 species in central and northern Europe. The comparison of the model predictions with the ground measurements in four measurement stations is encouraging. The model reproduces more than 94% of the daily averaged data and more than 87% of the hourly data within a factor of 2 for PM1 OA. The model tends to predict relatively flat diurnal profiles for PM1 OA in many areas, both rural and urban in agreement with the available measurements. The model performance against the high time resolution airborne measurements at multiple altitudes and locations is as good as its performance against the ground level hourly measurements. There is no evidence of missing sources of OA aloft over Europe during this period.

scholarly journals Evaluation of a three-dimensional chemical transport model (PMCAMx) in the European domain during the EUCAARI May 2008 campaign

2011 ◽  
Vol 11 (5) ◽  
pp. 14183-14220 ◽  
Author(s):  
C. Fountoukis ◽  
P. N. Racherla ◽  
H. A. C. Denier van der Gon ◽  
P. Polymeneas ◽  
P. E. Haralabidis ◽  
...  
Keyword(s):  
Time Resolution ◽  
Transport Model ◽  
Three Dimensional ◽  
Model Performance ◽  
Ground Level ◽  
Chemical Transport ◽  
Organic Aerosol ◽  
High Time Resolution ◽  
Chemical Transport Model ◽  
Airborne Measurements

Abstract. PMCAMx-2008, a detailed three dimensional chemical transport model (CTM), was applied to Europe to simulate the mass concentration and chemical composition of particulate matter (PM) during May 2008. The model includes a state-of-the-art organic aerosol module which is based on the volatility basis set framework treating both primary and secondary organic components to be semivolatile and photochemically reactive. The model performance is evaluated against high time resolution aerosol mass spectrometer (AMS) ground and airborne measurements. Overall, organic aerosol is predicted to account for 32% of total PM1 at ground level during May 2008, followed by sulfate (30%), crustal material and sea-salt (14%), ammonium (13%), nitrate (7%), and elemental carbon (4%). The model predicts that fresh primary OA (POA) is a small contributor to organic PM concentrations in Europe during late spring, and that oxygenated species (oxidized primary and biogenic secondary) dominate the ambient OA. The Mediterranean region is the only area in Europe where sulfate concentrations are predicted to be much higher than the OA, while organic matter is predicted to be the dominant PM1 species in Central and Northern Europe. The comparison of the model predictions with the ground measurements in four measurement stations is encouraging. The model reproduces more than 94% of the daily averaged data and more than 87% of the hourly data within a factor of 2 for PM1 OA. The model tends to predict relatively flat diurnal profiles for PM1 OA in many areas, both rural and urban, in agreement with the available measurements. The model performance against the high time resolution airborne measurements at multiple altitudes and locations is as good as its performance against the ground level hourly measurements. There is no evidence of missing sources of OA aloft over Europe during this period.

scholarly journals Evaluation of the volatility basis-set approach for the simulation of organic aerosol formation in the Mexico City metropolitan area

2010 ◽  
Vol 10 (2) ◽  
pp. 525-546 ◽  
Author(s):  
A. P. Tsimpidi ◽  
V. A. Karydis ◽  
M. Zavala ◽  
W. Lei ◽  
L. Molina ◽  
...  
Keyword(s):  
Mexico City ◽  
Metropolitan Area ◽  
Secondary Organic Aerosol ◽  
Transport Model ◽  
Three Dimensional ◽  
Organic Aerosol ◽  
Basis Set ◽  
Aerosol Formation ◽  
Chemical Transport Model ◽  
Starting Point

Abstract. New primary and secondary organic aerosol modules have been added to PMCAMx, a three dimensional chemical transport model (CTM), for use with the SAPRC99 chemistry mechanism based on recent smog chamber studies. The new modelling framework is based on the volatility basis-set approach: both primary and secondary organic components are assumed to be semivolatile and photochemically reactive and are distributed in logarithmically spaced volatility bins. This new framework with the use of the new volatility basis parameters for low-NOx and high-NOx conditions tends to predict 4–6 times higher anthropogenic SOA concentrations than those predicted with the older generation of models. The resulting PMCAMx-2008 was applied in Mexico City Metropolitan Area (MCMA) for approximately a week during April 2003 during a period of very low regional biomass burning impact. The emission inventory, which uses as a starting point the MCMA 2004 official inventory, is modified and the primary organic aerosol (POA) emissions are distributed by volatility based on dilution experiments. The predicted organic aerosol (OA) concentrations peak in the center of Mexico City, reaching values above 40 μg m−3. The model predictions are compared with the results of the Positive Matrix Factorization (PMF) analysis of the Aerosol Mass Spectrometry (AMS) observations. The model reproduces both Hydrocarbon-like Organic Aerosol (HOA) and Oxygenated Organic Aerosol (OOA) concentrations and diurnal profiles. The small OA underprediction during the rush-hour periods and overprediction in the afternoon suggest potential improvements to the description of fresh primary organic emissions and the formation of the oxygenated organic aerosols, respectively, although they may also be due to errors in the simulation of dispersion and vertical mixing. However, the AMS OOA data are not specific enough to prove that the model reproduces the organic aerosol observations for the right reasons. Other combinations of contributions of primary and secondary organic aerosol production rates may lead to similar results. The model results strongly suggest that, during the simulated period, transport of OA from outside the city was a significant contributor to the observed OA levels. Future simulations should use a larger domain in order to test whether the regional OA can be predicted with current SOA parameterizations. Sensitivity tests indicate that the predicted OA concentration is especially sensitive to the volatility distribution of the emissions in the lower volatility bins.

scholarly journals Sources and production of organic aerosol in Mexico City: insights from the combination of a chemical transport model (PMCAMx-2008) and measurements during MILAGRO

2011 ◽  
Vol 11 (11) ◽  
pp. 5153-5168 ◽  
Author(s):  
A. P. Tsimpidi ◽  
V. A. Karydis ◽  
M. Zavala ◽  
W. Lei ◽  
N. Bei ◽  
...  
Keyword(s):  
Mexico City ◽  
Biomass Burning ◽  
Urban Areas ◽  
Transport Model ◽  
Three Dimensional ◽  
Chemical Transport ◽  
Organic Aerosol ◽  
Basis Set ◽  
Chemical Transport Model ◽  
Aerosol Mass

Abstract. Urban areas are large sources of organic aerosols and their precursors. Nevertheless, the contributions of primary (POA) and secondary organic aerosol (SOA) to the observed particulate matter levels have been difficult to quantify. In this study the three-dimensional chemical transport model PMCAMx-2008 is used to investigate the temporal and geographic variability of organic aerosol in the Mexico City Metropolitan Area (MCMA) during the MILAGRO campaign that took place in the spring of 2006. The organic module of PMCAMx-2008 includes the recently developed volatility basis-set framework in which both primary and secondary organic components are assumed to be semi-volatile and photochemically reactive and are distributed in logarithmically spaced volatility bins. The MCMA emission inventory is modified and the POA emissions are distributed by volatility based on dilution experiments. The model predictions are compared with observations from four different types of sites, an urban (T0), a suburban (T1), a rural (T2), and an elevated site in Pico de Tres Padres (PTP). The performance of the model in reproducing organic mass concentrations in these sites is encouraging. The average predicted PM1 organic aerosol (OA) concentration in T0, T1, and T2 is 18 μg m−3, 11.7 μg m−3, and 10.5 μg m−3 respectively, while the corresponding measured values are 17.2 μg m−3, 11 μg m−3, and 9 μg m−3. The average predicted locally-emitted primary OA concentrations, 4.4 μg m−3 at T0, 1.2 μg m−3 at T1 and 1.7 μg m−3 at PTP, are in reasonably good agreement with the corresponding PMF analysis estimates based on the Aerosol Mass Spectrometer (AMS) observations of 4.5, 1.3, and 2.9 μg m−3 respectively. The model reproduces reasonably well the average oxygenated OA (OOA) levels in T0 (7.5 μg m−3 predicted versus 7.5 μg m−3 measured), in T1 (6.3 μg m−3 predicted versus 4.6 μg m−3 measured) and in PTP (6.6 μg m−3 predicted versus 5.9 μg m−3 measured). The rest of the OA mass (6.1 μg m−3 and 4.2 μg m−3 in T0 and T1 respectively) is assumed to originate from biomass burning activities and is introduced to the model as part of the boundary conditions. Inside Mexico City (at T0), the locally-produced OA is predicted to be on average 60 % locally-emitted primary (POA), 6 % semi-volatile (S-SOA) and intermediate volatile (I-SOA) organic aerosol, and 34 % traditional SOA from the oxidation of VOCs (V-SOA). The average contributions of the OA components to the locally-produced OA for the entire modelling domain are predicted to be 32 % POA, 10 % S-SOA and I-SOA, and 58 % V-SOA. The long range transport from biomass burning activities and other sources in Mexico is predicted to contribute on average almost as much as the local sources during the MILAGRO period.

scholarly journals Simulation of the evolution of biomass burning organic aerosol with different volatility basis set schemes in PMCAMx-SRv1.0

2020 ◽  
Author(s):  
Georgia N. Theodoritsi ◽  
Giancarlo Ciarelli ◽  
Spyros N. Pandis
Keyword(s):  
Biomass Burning ◽  
Transport Model ◽  
Three Dimensional ◽  
Organic Aerosol ◽  
Basis Set ◽  
Base Case ◽  
Chemical Transport Model ◽  
Alternative Scheme ◽  
Average Maximum ◽  
The Impact

Abstract. A source-resolved three-dimensional chemical transport model, PMCAMx-SR, was applied in the continental U.S. to investigate the contribution of the various components (primary and secondary) of biomass burning organic aerosol (bbOA) to organic aerosol levels. Two different schemes based on the volatility basis set were used for the simulation of the bbOA during different seasons. The first is the default scheme of PMCAMx-SR and the second is a recently developed scheme based on laboratory experiments of the bbOA evolution. The simulations with the alternative bbOA scheme predict much higher total bbOA concentrations when compared with the base case ones. This is mainly due to the high emissions of intermediate volatility organic compounds (IVOCs) assumed in the alternative scheme. The oxidation of these compounds is predicted to be a significant source of secondary organic aerosol. The impact of the other parameters that differ in the two schemes is low to negligible. The monthly average maximum predicted concentrations of the alternative bbOA scheme were approximately an order of magnitude higher than those of the default scheme during all seasons. The performance of the two schemes was evaluated against observed total organic aerosol concentrations from several measurement sites across the US. The results were mixed. The default scheme performed better during July and September while the alternative scheme performed a little better during April. These results illustrate the uncertainty of the corresponding predictions, the need to quantify the emissions and reactions of IVOCs from specific biomass sources, and to better constrain the total (primary and secondary) bbOA levels.

scholarly journals Sources and production of organic aerosol in Mexico City: insights from the combination of a chemical transport model (PMCAMx-2008) and measurements during MILAGRO

2010 ◽  
Vol 10 (11) ◽  
pp. 27925-27965
Author(s):  
A. P. Tsimpidi ◽  
V. A. Karydis ◽  
M. Zavala ◽  
W. Lei ◽  
N. Bei ◽  
...  
Keyword(s):  
Mexico City ◽  
Urban Areas ◽  
Transport Model ◽  
Three Dimensional ◽  
Chemical Transport ◽  
Organic Aerosol ◽  
Basis Set ◽  
Chemical Transport Model ◽  
Range Transport ◽  
Dilution Experiments

Abstract. Urban areas are large sources of organic aerosols and their precursors. Nevertheless, the contributions of primary (POA) and secondary organic aerosol (SOA) to the observed particulate matter levels have been difficult to quantify. In this study the three-dimensional chemical transport model PMCAMx-2008 is used to investigate the temporal and geographic variability of organic aerosol in the Mexico City Metropolitan Area (MCMA) during the MILAGRO campaign that took place in the spring of 2006. The organic module of PMCAMx-2008 is based on the volatility basis-set approach: both primary and secondary organic components are assumed to be semi-volatile and photochemically reactive and are distributed in logarithmically spaced volatility bins. The MCMA emission inventory is modified and the POA emissions are distributed by volatility based on dilution experiments. The model predictions are compared with observations from four different types of sites, an urban (T0), a suburban (T1), a rural (T2), and an elevated site in Pico Tres Padres (PTP). The performance of the model in reproducing organic mass concentrations in these sites was encouraging. The average predicted PM1 OA concentration in T0, T1, and T2 was 18 μg m−3, 11.7 μg m−3, and 10.5 μg m−3 respectively, while the corresponding measured values were 17.2 μg m−3, 11 μg m−3, and 9 μg m−3. The average predicted fresh primary OA concentrations were 4.4 μg m−3 at T0, 1.2 μg m−3 at T1 and 1.7 μg m−3 at PTP in reasonably good agreement with the corresponding PMF analysis estimates based on the AMS observations of 4.5, 1.3, and 2.9 μg m−3 respectively. The model reproduced reasonably well the average oxygenated OA (OOA) levels in T0 (7.5 μg m−3 predicted versus 7.5 μg m−3 measured), in T1 (6.3 μg m−3 predicted versus 4.6 μg m−3 measured) and in PTP (6.6 μg m−3 predicted versus 5.9 μg m−3 measured). Inside Mexico City, the locally produced OA is predicted to be on average 53% fresh primary (POA), 11% semi-volatile (S-SOA) and intermediate volatile (I-SOA) organic aerosol, and 36% traditional SOA from the oxidation of VOCs (V-SOA). The long range transport from biomass burning activities and other sources in Mexico is predicted to contribute on average almost as much as the local sources during the MILAGRO period.

scholarly journals The UIUC three-dimensional stratospheric chemical transport model: Description and evaluation of the simulated source gases and ozone

1999 ◽  
Vol 104 (D9) ◽  
pp. 11755-11781 ◽  
Author(s):  
Eugene V. Rozanov ◽  
Vladimir A. Zubov ◽  
Michael E. Schlesinger ◽  
Fanglin Yang ◽  
Natalia G. Andronova
Keyword(s):  
Transport Model ◽  
Three Dimensional ◽  
Chemical Transport ◽  
Model Description ◽  
Chemical Transport Model ◽  
Simulated Source

scholarly journals Implementation of state-of-the-art ternary new-particle formation scheme to the regional chemical transport model PMCAMx-UF in Europe

2016 ◽  
Vol 9 (8) ◽  
pp. 2741-2754 ◽  
Author(s):  
Elham Baranizadeh ◽  
Benjamin N. Murphy ◽  
Jan Julin ◽  
Saeed Falahat ◽  
Carly L. Reddington ◽  
...  
Keyword(s):  
Transport Model ◽  
Three Dimensional ◽  
Chemical Transport ◽  
Particle Formation ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
New Particle Formation ◽  
Chemical Transport Model ◽  
Order Of Magnitude ◽  
Adjustment Scheme

Abstract. The particle formation scheme within PMCAMx-UF, a three-dimensional chemical transport model, was updated with particle formation rates for the ternary H2SO4–NH3–H2O pathway simulated by the Atmospheric Cluster Dynamics Code (ACDC) using quantum chemical input data. The model was applied over Europe for May 2008, during which the EUCAARI-LONGREX (European Aerosol Cloud Climate and Air Quality Interactions–Long-Range Experiment) campaign was carried out, providing aircraft vertical profiles of aerosol number concentrations. The updated model reproduces the observed number concentrations of particles larger than 4 nm within 1 order of magnitude throughout the atmospheric column. This agreement is encouraging considering the fact that no semi-empirical fitting was needed to obtain realistic particle formation rates. The cloud adjustment scheme for modifying the photolysis rate profiles within PMCAMx-UF was also updated with the TUV (Tropospheric Ultraviolet and Visible) radiative-transfer model. Results show that, although the effect of the new cloud adjustment scheme on total number concentrations is small, enhanced new-particle formation is predicted near cloudy regions. This is due to the enhanced radiation above and in the vicinity of the clouds, which in turn leads to higher production of sulfuric acid. The sensitivity of the results to including emissions from natural sources is also discussed.

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